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Chemical Physics

Interaction between excitons determines the non-linear response of nanocrystals

Mayrose R. Salvador, P. Sreekumari Nair, Minhaeng Cho, Gregory D. Scholes

Published Jan 15, 2008• 19 citations
Publisher
DOI
10.1016/j.chemphys.2007.12.020

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We show that the exciton–exciton scattering continuum has a significant influence on the transient non-linear optical response of semiconductor microcavities. Comparison between transient shifts observed in pump and probe experiments and calculations demonstrates almost complete cancellation between mean-field and two-exciton continuum contributions. Moreover, we show that suppression of non-linear absorption of the lower polariton observed in many experiments is determined by the specific spectral shape of these correlations. In particular, we find that the pump induced dephasing of polariton resonances is proportional to the spectrum of four-particle correlations calculated at the energy sum of the pumped and probed polaritons.
The nonlinear optical response of interacting charge-transfer excitons is investigated theoretically by means of pseudospin operators for the model Hamiltonian. The generalized optical Bloch equations including the static dipolar interaction of charge-transfer excitons are derived in terms of the Heisenberg equation of motion and the mean-field approximation. It is shown that the intrinsic optical bistability due to the strong interaction of charge-transfer excitons may exist in the interacting charge-transfer exciton system. The absorption spectrum of interacting charge-transfer excitons associated with a weak probe field in the presence of a strong pump field is also calculated using the linear-response theory. The results show that a gain without population inversion can be observed in the interacting charge-transfer exciton system.
In recent years, non-linear optical phenomena have attracted much attention, with a particular focus on the engineering and exploitation of non-linear responses. Comparatively little study has however been devoted to the driving fields that generate these responses. In this work, we demonstrate that the relationship between a driving field and the optical response it induces is non-unique. Using a generic model for a strongly interacting system, we show that multiple candidate driving field exists, which will all generate the same response. Consequently, it is possible show that the optical response is not sufficient to determine the internal dynamics of the system, and that different solutions for the driving field will do different amounts of work on a system. This non-uniqueness phenomenon may in future be utilised to engineer internal system states without modifying its optical response.